Reactive barriers for Cs retention

¹³⁷Cs was dispersed globally by cold war activities and, more recently, by the Chernobyl accident. Engineered extraction of ¹³⁷Cs from soils and groundwaters is exceedingly difficult. Because the half-life of ¹³⁷Cs is only 30.2 years, remediation might be more effective (and less costly) if ¹³⁷Cs bioavailability could be demonstrably limited for even a few decades by use of a reactive barrier. Essentially permanent isolation must be demonstrated in those few settings where high nuclear level wastes contaminated the environment with ¹³⁵Cs (half-life 2.3×10⁶ years) in addition to ¹³⁷Cs. Clays are potentially a low-cost barrier to Cs movement, though their long-term effectiveness remains untested. To identify optimal clays for Cs retention, Cs desorption was measured for five common clays: Wyoming Montmorillonite (SWy-1), Georgia Kaolinites (KGa-1 and KGa-2), Fithian Illite (F-Ill), and K-Metabentonite (K-Mbt). Exchange sites were pre-saturated with 0.16 M CsCl for 14 days and readily exchangeable Cs was removed by a series of LiNO₃ and LiCl washes. Washed clays were then placed into dialysis bags and the Cs release to the deionized water outside the bags measured. Release rates from 75 to 139 days for SWy-1, K-Mbt and F-Ill were similar; 0.017% to 0.021% sorbed Cs released per day. Both kaolinites released Cs more rapidly (0.12% to 0.05% of the sorbed Cs per day). In a second set of experiments, clays were Cs-doped for 110 days and subjected to an extreme and prolonged rinsing process. All the clays exhibited some capacity for irreversible Cs uptake. However, the residual loading was greatest on K-Mbt (0.33 wt.% Cs). Thus, this clay would be the optimal material for constructing artifical reactive barriers.     

Distribution coefficients (Kd) and desorption rates of Cs and Am in Black Sea sediments

The distribution coefficients (K_d) and desorption rates of ¹³⁷Cs and ²⁴¹Am radionuclides in bottom sediments at different locations in the Black Sea were studied under laboratory conditions. The K_d values were found to be 500 for ¹³⁷Cs and 3800 for ²⁴¹Am at the steady state and described exponential curves. Rapid uptake of the radionuclides occurred during the initial period and little accumulation happened after four days. The desorption rates for ¹³⁷Cs in different bottom sediments were best described by a three-component exponential model. The desorption half-times of ¹³⁷Cs ranged from 26 to 50 d at the slow components. However, the desorption rate of ²⁴¹Am described one component for all sediment samples and desorption half-time was found to be 75 d. In general, the results showed that the ²⁴¹Am radionuclide is more effectively transferred to bottom sediment and has longer turnover time than ¹³⁷Cs under Black Sea conditions.     

PERSISTING SEDIMENT YIELDS AND SEDIMENT DELWERY CHANGES1

ABSTRACT: The Buffalo River is a tributary to the Mississippi River in west-central Wisconsin that drains a watershed dominated by agricultural land uses. Since 1935, backwater from Lock and Dam 4 on the Mississippi River has inundated the mouth of the Buffalo's valley. Resurveys of a transect first surveyed across the lake in 1935 and cesium-137 dating of backwater sediments reveal that sedimentation rates at the Buffalo's mouth have remained unchanged since the mid-1940s. Study results indicate that sediment yields from the watershed have persisted at relatively high levels over a period of several decades despite pronounced trends toward less cultivated land and major efforts to control soil erosion from agricultural land. The maintenance of sediment yields is probably due to increased channel conveyance capacities resulting from incision along some tributary streams since the early 1950s. Post-1950 incision extended the network of historical incised tributary channels, enhancing the efficient delivery of sediment from upland sources to downstream sites.     

Transfer of Cs into fish in small forest lakes

The transfer of ¹³⁷Cs into fish in seepage and drainage lakes from 1988 to 1992 was analysed using linear regression. Empirical results for ¹³⁷Cs in lake water and fish were used to calculate concentration factors (CFs). In the drainage lakes the CF decreased during the study period by 9% per year whereas in the seepage lakes the CF increased significantly by 4.3% per year. The transfer of ¹³⁷Cs into pike was significantly (1.6 times) higher than that into perch. The CF increased on average by 3.4% for each 1-cm increase in the median size of perch. The relationship between the water chemistry and the CF differed between clear-water seepage and brown-water drainage lakes.     

C, δC and total C content in soils around a Brazilian PWR nuclear power plant

Nuclear power plants release ¹⁴C during routine operation mainly as airborne gaseous effluents. Because of the long half-life (5730 years) and biological importance of this radionuclide (it is incorporated in plant tissue by photosynthesis), several countries have monitoring programs in order to quantify and control these emissions. This paper compares the activity of ¹⁴C in soils taken within 1 km from a Brazilian nuclear power plant with soils taken within a reference area located 50 km away from the reactor site. Analyses of total carbon, δ¹³C and ¹³⁷Cs were also performed in order to understand the local soil dynamics. Except for one of the profiles, the isotopic composition of soil organic carbon reflected the actual forest vegetation present in both areas. The ¹³⁷Cs data show that the soils from the base of hills are probably allocthonous.     

Medical radioisotopes in the environment – following the pathway from patient to river sediment

Motivated by the detection of ¹³¹I in river sediment in routine long-term surveillance samples, a systematic short-term study of the wastewater treatment chain was planned and conducted. Inflow, effluent and primary sludge were collected on a daily basis during two weeks at a regional wastewater treatment plant. Samples were investigated by gamma spectroscopy. Four medically used isotopes could be identified (¹³¹I and ^99mTc regularly, ¹⁵³Sm and ¹²³I sporadically). The concentration levels coincide well with literature data for ¹³¹I, and with our own long-term data for ¹³¹I and ^99mTc for the same plant. Cosmogenic ⁷Be activity in primary sludge correlated well with rainfall intensity. Surface sediment was sampled at low tide at both shores of the river, up- and downstream of the plant. ¹³¹I was identified in all samples, with a sharp maximum (about 100 Bq kg⁻¹ d.m.) at the discharge point of the plant and lower levels elsewhere, decreasing monotonically in downstream direction. ⁷Be and ¹³⁷Cs showed the same behaviour, but no peak at the discharge point. Predictions from simple equilibrium models for the transport and sedimentation of ¹³¹I show good agreement with the experimental data and suggest that the wastewater treatment plant is the main source for this isotope.     

Preliminary Caesium Data From A Cooperative Us/Ussr Monitoring Survey for Chernobyl Radioactivity in the Black Sea

In June 1990, scientists from the US Environmental Protection Agency's (EPA) Office of Radiation Programs (ORP), and the Woods Hole Oceanographic Institution (WHOI), travelled to Sevastopol in the Soviet Union to work with radioecologists and marine scientists from the USSR Institute of Biology of the Southern Seas (IBSS). the purpose of this cooperative programme was to conduct a monitoring survey for radioactivity in the northwestern Black Sea. Samples of sediment, surface and in-situ water, and biota were collected from fourteen stations for post-survey radionuclide analyses to determine levels of radioactivity in the Black Sea environment resulting from the Chernobyl nuclear power plant explosion and subsequent transport of radioactivity via the Dnepr and Danube rivers. This paper presents the preliminary data for caesium-137 and caesium-134 in sediment samples analyzed by the EPA/ORP. Caesium-137 was measured at four shallow (20–114 m) stations on the shelf near the mouth of the Dnepr and Danube Rivers, but was not detected in sediments from comparable depths at stations further off shore or in slope sediments at depths of 510–1288 meters. Caesium-134 was detected only in sediments from the shallow-water station nearest to the Danube River.     

Retention of 137cesium in acid sulphate soils of South Central Thailand

Adsorption and desorption of ¹³⁷Cs by acid sulphate soils from the Nakhon Nayok province, South Central Plain of Thailand located near the Ongkarak Nuclear Research Center (ONRC) were investigated using a batch equilibration technique. The influence of added limestone (12 and 18 tons ha^?1) on ¹³⁷Cs adsorption–desorption was studied. Based on Freundlich isotherms, both adsorption and desorption of ¹³⁷Cs were nonlinear. A large portion (98.26–99.97%) of added ¹³⁷Cs (3.7?×?10³?7.03?×?10⁵ Bq l^?1) was sorbed by the soils with or without added lime. The higher lime treatments, however, favoured stronger adsorption of ¹³⁷Cs as compared with soil with no lime, which was supported by higher K _ads values. The addition of lime, the cation exchange capacity and pH of the soil increased and hence favoured the stronger adsorption of ¹³⁷Cs. Acid sulphate soils with a high clay content, medium to high organic matter, high CEC, and predominant clay types consisting of a mixture of illite, kaolinite, and montmorillonite were the main soil factors contributing to the high ¹³⁷Cs adsorption capacity. Competing cations such as NH₄ ⁺, K⁺, Na⁺, Ca²⁺, and Mg²⁺ had little influence on ¹³⁷Cs adsorption as compared with liming, where a significant positive correlation between K _ads and soil pH was observed. The ¹³⁷Cs adsorption–desorption characteristics of the acid sulphate soils studied exhibited a very strong irreversible sorption pattern. Only a small portion (0.09–0.58%) of ¹³⁷Cs adsorbed at the highest added initial ¹³⁷Cs concentration was desorbed by four successive soil extractions. Results clearly demonstrated that Nakhon Nayok province acid sulphate soils have a high ¹³⁷Cs adsorption capacity, which limits the ¹³⁷Cs bioavailability.     

Retention of 137cesium in acid sulphate soils of South Central Thailand

Adsorption and desorption of ¹³⁷Cs by acid sulphate soils from the Nakhon Nayok province, South Central Plain of Thailand located near the Ongkarak Nuclear Research Center (ONRC) were investigated using a batch equilibration technique. The influence of added limestone (12 and 18 tons ha^-1) on ¹³⁷Cs adsorption-desorption was studied. Based on Freundlich isotherms, both adsorption and desorption of ¹³⁷Cs were nonlinear. A large portion (98.26-99.97%) of added ¹³⁷Cs (3.7 × 10³-7.03 × 10⁵ Bq l^-1) was sorbed by the soils with or without added lime. The higher lime treatments, however, favoured stronger adsorption of ¹³⁷Cs as compared with soil with no lime, which was supported by higher K_ads values. The addition of lime, the cation exchange capacity and pH of the soil increased and hence favoured the stronger adsorption of ¹³⁷Cs. Acid sulphate soils with a high clay content, medium to high organic matter, high CEC, and predominant clay types consisting of a mixture of illite, kaolinite, and montmorillonite were the main soil factors contributing to the high ¹³⁷Cs adsorption capacity. Competing cations such as NH₄⁺, K⁺, Na⁺, Ca²⁺, and Mg²⁺ had little influence on ¹³⁷Cs adsorption as compared with liming, where a significant positive correlation between K_ads and soil pH was observed. The ¹³⁷Cs adsorption-desorption characteristics of the acid sulphate soils studied exhibited a very strong irreversible sorption pattern. Only a small portion (0.09-0.58%) of ¹³⁷Cs adsorbed at the highest added initial ¹³⁷Cs concentration was desorbed by four successive soil extractions. Results clearly demonstrated that Nakhon Nayok province acid sulphate soils have a high ¹³⁷Cs adsorption capacity, which limits the ¹³⁷Cs bioavailability.